Adatom Bonding Sites in a Nickel-Fe 3 O 4 (001) Single-Atom Model Catalyst and O 2 Reactivity Unveiled by Surface Action Spectroscopy with Infrared Free-Electron Laser Light.

Autor: Liu Y; Department of Interface Science, Fritz-Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany., Han Z; Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Bolshoy Blvd. 30/1, 121205, Moscow, Russia., Gewinner S; Molecular Physics Department, Fritz-Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany., Schöllkopf W; Molecular Physics Department, Fritz-Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany., Levchenko SV; Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Bolshoy Blvd. 30/1, 121205, Moscow, Russia., Kuhlenbeck H; Department of Interface Science, Fritz-Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany., Roldan Cuenya B; Department of Interface Science, Fritz-Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2022 Jul 11; Vol. 61 (28), pp. e202202561. Date of Electronic Publication: 2022 May 19.
DOI: 10.1002/anie.202202561
Abstrakt: Single-atom (SA) catalysis presently receives much attention with its promise to decrease the cost of the active material while increasing the catalyst's performance. However, key details such as the exact location of SA species and their stability are often unclear due to a lack of atomic level information. Here, we show how vibrational spectra measured with surface action spectroscopy (SAS) and density functional theory (DFT) simulations can differentiate between different adatom binding sites and determine the location of Ni and Au single atoms on Fe 3 O 4 (001). We reveal that Ni and Au adatoms selectively bind to surface oxygen ions which are octahedrally coordinated to Fe ions. In addition, we find that the Ni adatoms can activate O 2 to superoxide in contrast to the bare surface and Ni in subsurface positions. Overall, we unveil the advantages of combining SAS and DFT for improving the understanding of single-atom catalysts.
(© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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